Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator

Ruihuan Duan; Song Zhu; Xiaodong Xu; Yao Wu; Sicheng Zhou; Xuan Mao; Zhen Xu; Wenduo Chen; Xiaodan Lyu; Youqiang Huang; Yi Zhang; Fakun Wang; Lishu Wu; Ya Deng; Manzhang Xu; Yanchao He; Jiayu Shi; Wenting Zhao; Guangtong Liu; Weibo Gao; Zhipei Sun; Xingji Li; Qi Jie Wang; Zheng Liu

doi:10.1038/s41377-025-02130-3

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Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator

Original Articles

- Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator
- Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator
- Light: Science & Applications 2026年15卷第2期页码：647-657
- Affiliations：
  
  1.School of Materials Science and Engineering, Nanyang Technological University, 639798 Singapore, Singapore
  2.School of Electrical and Electronic Engineering, Nanyang Technological University, 639798 Singapore, Singapore
  3.National Key Laboratory of Microwave Photonics, Nanjing University of Aeronautics and Astronautics, Nanjing, China
  4.School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China
  5.Beijing National Laboratory of Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, 100190 Beijing, China
  6.School of Physical and Mathematical Sciences, Nanyang Technological University, 637371 Singapore, Singapore
  7.Department of Electronics and Nanoengineering and QTF Centre of Excellence, Aalto University, Aalto, Finland
  8.Frontiers Science Center for Flexible Electronics (FSCFE) & Institute of Flexible Electronics (IFE), Northwestern Polytechnical University, Xi'an 710072, China
- Author bio：
  
  Xingji Li (lxj0218@hit.edu.cn)
  Qi Jie Wang (qjwang@ntu.edu.sg)
  Zheng Liu (z.liu@ntu.edu.sg)
- Funds：
- DOI：10.1038/s41377-025-02130-3
  中图分类号：
- 收稿：2025-03-22，
  
  修回：2025-09-02，
  
  录用：2025-11-07，
  
  网络首发：2026-01-08，
  
  纸质出版：2026-02-28
- Accepted：
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Ruihuan Duan, Song Zhu, Xiaodong Xu, 等. Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator[J]. Light: Science & Applications, 2026,15(2):647-657.

Duan, R. H. et al. Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator. Light: Science & Applications, 15, 647-657 (2026).
Ruihuan Duan, Song Zhu, Xiaodong Xu, 等. Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator[J]. Light: Science & Applications, 2026,15(2):647-657. DOI： 10.1038/s41377-025-02130-3.

Duan, R. H. et al. Colossal infrared nonlinear optical anisotropy in a 2D charge-transfer Mott insulator. Light: Science & Applications, 15, 647-657 (2026). DOI： 10.1038/s41377-025-02130-3.

摘要

Abstract

Mott insulators are a unique class of materials whose insulating state originates from strong electron-electron correlations: the interactions localize charge carriers

and the resulting on-site Coulomb repulsion opens a charge gap

fundamentally different from conventional insulators

making these systems an exceptional platform for exploring exotic physical phenomena. Significantly

the interplay between strong correlations and charge transfer not only stabilizes the antiferromagnetic ground state but also endows the material with enriched properties

particularly in optics. Herein

we demonstrate a 2D antiferromagnetic charge-transfer Mott insulator

Vanadium Oxychloride (VOCl)

which shows giant third-harmonic generation (THG) anisotropy (

THG

where

and

represent the THG intensities corresponding to the excitation polarization parallel to crystal's

- and

-axes)

with

THG

reaching up to 187 at 1280 nm excitation wavelength. Notably

it is the highest THG anisotropic ratio within the van der Waals materials family. The nonlinear anisotropy is further modulated across a broadband infrared (IR) excitation wavelength range from 2028 to 1280 nm

during which

THG

rises from 2.6 to 187

corresponding to a 72-fold enhancement relative to its value at 2028 nm. Additionally

VOCl demonstrates layer-independent third-order susceptibilities (χ

(3)

~ 10

-19

) and band structures attributed to its extremely weak interlayer electronic coupling. Moreover

the colossal THG anisotropic ratio in 2D VOCl can be ascribed to the synergistic effect of the correlated charge-transfer Mott insulator behavior and intrinsic

symmetry breaking

as supported by theoretical calculations. The colossal nonlinear optical anisotropy in 2D VOCl positions it as an excellent candidate for nanophotonic and optoelectronic applications

enabling next-generation nanodevices based on 2D correlated Mott insulators.

关键词

Keywords

references

Yue, L. et al. Giant nonlinear optical wave mixing in a van der Waals correlated insulator. Sci. Adv. 10 , eadn6216 (2024)..

Zhu, S. et al. Strong nonlinear optical processes with extraordinary polarization anisotropy in inversion-symmetry broken two-dimensional PdPSe. Light Sci. Appl. 13 , 119 (2024)..

Guo, Q. B. et al. Colossal in-plane optical anisotropy in a two-dimensional van der Waals crystal. Nat. Photonics 18 , 1170–1175 (2024)..

Zhou, Y. et al. A solution-processable natural crystal with giant optical anisotropy for efficient manipulation of light polarization. Nat. Photonics 18 , 922–927 (2024)..

Autere, A. et al. Nonlinear optics with 2D layered materials. Adv. Mater. 30 , 1705963 (2018)..

Ma, R., Sutherland, D. S. & Shi, Y. M. Harmonic generation in transition metal dichalcogenides and their heterostructures. Mater. Today 50 , 570–586 (2021)..

Xie, Z. X. et al. Nonlinear optical properties of 2D materials and their applications. Small 20 , 2311621 (2024)..

Nicholls, L. H. et al. Ultrafast synthesis and switching of light polarization in nonlinear anisotropic metamaterials. Nat. Photonics 11 , 628–633 (2017)..

Wu, L. et al. Giant anisotropic nonlinear optical response in transition metal monopnictide Weyl semimetals. Nat. Phys. 13 , 350–355 (2017)..

Niu, S. Y. et al. Giant optical anisotropy in a quasi-one-dimensional crystal. Nat. Photonics 12 , 392–396 (2018)..

Zhang, H. Q. et al. Cavity-enhanced linear dichroism in a van der Waals antiferromagnet. Nat. Photonics 16 , 311–317 (2022)..

Wu, C. et al. Giant optical anisotropy in the UV-transparent 2D nonlinear optical material Sc(IO 3 ) 2 (NO 3 ). Angew. Chem. Int. Ed. 60 , 3464–3468 (2021)..

Li, X. et al. Review of anisotropic 2D materials: controlled growth, optical anisotropy modulation, and photonic applications. Laser Photonics Rev. 15 , 2100322 (2021)..

Ermolaev, G. A. et al. Giant optical anisotropy in transition metal dichalcogenides for next-generation photonics. Nat. Commun. 12 , 854 (2021)..

Du, L. J. et al. Giant anisotropic photonics in the 1D van der Waals semiconductor fibrous red phosphorus. Nat. Commun. 12 , 4822 (2021)..

Ghosh, H. Excited state nonlinear optics of quasi-one-dimensional Mott-Hubbard insulators. Phys. Rev. B 75 , 235127 (2007)..

Kishida, H. et al. Gigantic optical nonlinearity in one-dimensional Mott–Hubbard insulators. Nature 405 , 929–932 (2000)..

Murakami, Y. et al. Anomalous temperature dependence of high-harmonic generation in Mott insulators. Phys. Rev. Lett. 129 , 157401 (2022)..

Uchida, K. et al. High-order harmonic generation and its unconventional scaling law in the Mott-insulating Ca 2 RuO 4 . Phys. Rev. Lett. 128 , 127401 (2022)..

Hubbard, J. Electron correlations in narrow energy bands. Proc. R. Soc. A 276 , 238–257 (1963)..

Imada, M., Fujimori, A. & Tokura, Y. Metal-insulator transitions. Rev. Mod. Phys. 70 , 1039–1263 (1998)..

Takahashi, M., Tohyama, T. & Maekawa, S. Nonlinear optical response in two-dimensional Mott insulators. Phys. Rev. B 66 , 125102 (2002)..

Ono, M. et al. Linear and nonlinear optical properties of one-dimensional Mott insulators consisting of Ni-halogen chain and CuO-chain compounds. Phys. Rev. B 70 , 085101 (2004)..

Zhang, G. P. Origin of giant optical nonlinearity in charge-transfer-Mott insulators: a new paradigm for nonlinear optics. Phys. Rev. Lett. 86 , 2086–2089 (2001)..

Boyd, R. W. Nonlinear Optics . https://doi.org/10.1016/C2015-0-05510-1 https://doi.org/10.1016/C2015-0-05510-1 (Academic, 2020)..

Li, G. C. et al. Light-induced symmetry breaking for enhancing second-harmonic generation from an ultrathin plasmonic nanocavity. Nat. Commun. 12 , 4326 (2021)..

Glawion, S. et al. Electronic structure of the two-dimensional Heisenberg antiferromagnet VOCl: a multiorbital Mott insulator. Phys. Rev. B 80 , 155119 (2009)..

Villalpando, G. et al. Chemical exfoliation toward magnetic 2D VOCl monolayers. ACS Nano 16 , 13814–13820 (2022)..

Zhu, S. et al. Ultrastrong optical harmonic generations in layered platinum disulfide in the mid-infrared. ACS Nano 17 , 2148–2158 (2023)..

Autere, A. et al. Rapid and large-area characterization of exfoliated black phosphorus using third-harmonic generation microscopy. J. Phys. Chem. Lett. 8 , 1343–1350 (2017)..

Woodward, R. I. et al. Characterization of the second- and third-order nonlinear optical susceptibilities of monolayer MoS 2 using multiphoton microscopy. 2D Mater. 4 , 011006 (2017)..

Autere, A. et al. Optical harmonic generation in monolayer group-Ⅵ transition metal dichalcogenides. Phys. Rev. B 98 , 115426 (2018)..

Zhu, W. et al. Ternary VOCl single-crystal as efficient gate dielectric for 2D field-effect transistors. 2D Mater. 8 , 025010 (2021)..

Oyedele , A. D. et al. PdSe 2 : pentagonal two-dimensional layers with high air stability for electronics. J. Am. Chem. Soc. 139 , 14090–14097 (2017)..

Yu, X. C. et al. Atomically thin noble metal dichalcogenide: a broadband mid-infrared semiconductor. Nat. Commun. 9 , 1545 (2018)..

Das, S. et al. Tunable transport gap in phosphorene. Nano Lett. 14 , 5733–5739 (2014)..

Zaanen, J., Sawatzky, G. A. & Allen, J. W. Band gaps and electronic structure of transition-metal compounds. Phys. Rev. Lett. 55 , 418–421 (1985)..

Gao, S. Y. et al. Discovery of a single-band Mott insulator in a van der Waals flat-band compound. Phys. Rev. X 13 , 041049 (2023)..

Tang, E. et al. High-temperature fractional quantum Hall states. Phys. Rev. Lett. 106 , 236802 (2011)..

Du, L. J. et al. Engineering symmetry breaking in 2D layered materials. Nat. Rev. Phys. 3 , 193–206 (2021)..

Cai, H. et al. Synthesis of highly anisotropic semiconducting GaTe nanomaterials and emerging properties enabled by epitaxy. Adv. Mater. 29 , 1605551 (2017)..

Aslan, B. et al. Linearly polarized excitons in single- and few-layer ReS 2 crystals. ACS Photonics 3 , 96–101 (2016)..

Khatibi, A. et al. Anisotropic infrared light emission from quasi-1D layered TiS 3 . 2D Mater. 7 , 015022 (2020)..

Zhou, Z. Q. et al. Perpendicular optical reversal of the linear dichroism and polarized photodetection in 2D GeAs. ACS Nano 12 , 12416–12423 (2018)..

Yang, X. L. & Xie, S. W. Expression of third-order effective nonlinear susceptibility for third-harmonic generation in crystals. Appl. Opt. 34 , 6130–6135 (1995)..

Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77 , 3865–3868 (1996)..

Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54 , 11169–11186 (1996)..

Kresse, G. & Furthmüller, J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Computational Mater. Sci. 6 , 15–50 (1996)..

Klimeš, J., Bowler, D. R. & Michaelides, A. Chemical accuracy for the van der Waals density functional. J. Phys. : Condens. Matter 22 , 022201 (2010)..

Klimeš, J., Bowler, D. R. & Michaelides, A. Van der Waals density functionals applied to solids. Phys. Rev. B 83 , 195131 (2011)..

Marzari, N. et al. Maximally localizedWannier functions: theory and applications. Rev. Mod. Phys. 84 , 1419–1475 (2012)..

Aversa, C. & Sipe, J. E. Nonlinear optical susceptibilities of semiconductors: results with a length-gauge analysis. Phys. Rev. B 52 , 14636–14645 (1995)..

Xia, C. S. et al. Strong anisotropic third-harmonic generation in layered violet phosphorus. Nanoscale 16 , 11663–11668 (2024)..

Maragkakis, G. M. et al. Anisotropic third harmonic generation in 2D tin sulfide. Adv. Optical Mater. 12 , 2401321 (2024)..

Sar, H., Gao, J. & Yang, X. D. 2D layered SiP as anisotropic nonlinear optical material. Sci. Rep. 11 , 6372 (2021)..

Dasgupta, A., Gao, J. & Yang, X. D. Anisotropic third-harmonic generation in layered germanium selenide. Laser Photonics Rev. 14 , 1900416 (2020)..

Cui, Q. N. et al. Strong and anisotropic third-harmonic generation in monolayer and multilayer ReS 2 . Phys. Rev. B 95 , 165406 (2017)..

Sar, H., Gao, J. & Yang, X. D. In-plane anisotropic third-harmonic generation from germanium arsenide thin flakes. Sci. Rep. 10 , 14282 (2020)..

Youngblood, N. et al. Layer-tunable third-harmonic generation in multilayer black phosphorus. ACS Photonics 4 , 8–14 (2017)..

Dasgupta, A., Gao, J. & Yang, X. D. Natural van der Waals heterostructure cylindrite with highly anisotropic optical responses. npj 2D Mater. Appl. 5 , 74 (2021)..

Dasgupta, A., Yang, X. D. & Gao, J. Naturally occurring van der Waals heterostructure lengenbachite with strong in-plane structural and optical anisotropy. npj 2D Mater. Appl. 5 , 88 (2021)..

Tripathi, R. P. N., Yang, X. D. & Gao, J. Van der Waals layered mineral getchellite with anisotropic linear and nonlinear optical responses. Laser Photonics Rev. 15 , 2100182 (2021)..

Tripathi, R. P. N., Gao, J. & Yang, X. D. Naturally occurring layered mineral franckeite with anisotropic Raman scattering and third-harmonic generation responses. Sci. Rep. 11 , 8510 (2021)..

Dasgupta, A. et al. Large in-plane vibrational and optical anisotropy in natural 2D heterostructure abramovite. Sci. Rep. 12 , 16803 (2022)..

Chen, Z. H. et al. In-plane anisotropic nonlinear optical properties of two-dimensional organic–inorganic hybrid perovskite. J. Phys. Chem. Lett. 12 , 7010–7018 (2021)..

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